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Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol

Author

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  • Sebastian Grundner

    (Technische Universität München)

  • Monica A.C. Markovits

    (Technische Universität München)

  • Guanna Li

    (Schuit Institute of Catalysis, Inorganic Materials Chemistry Group, Eindhoven University of Technology)

  • Moniek Tromp

    (Van’t Hoff Institute for Molecular Sciences, University of Amsterdam)

  • Evgeny A. Pidko

    (Schuit Institute of Catalysis, Inorganic Materials Chemistry Group, Eindhoven University of Technology
    Institute for Complex Molecular Systems, Eindhoven University of Technology)

  • Emiel J.M. Hensen

    (Schuit Institute of Catalysis, Inorganic Materials Chemistry Group, Eindhoven University of Technology)

  • Andreas Jentys

    (Technische Universität München)

  • Maricruz Sanchez-Sanchez

    (Technische Universität München)

  • Johannes A. Lercher

    (Technische Universität München
    Institute for Integrated Catalysis, Pacific Northwest National Laboratory)

Abstract

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.

Suggested Citation

  • Sebastian Grundner & Monica A.C. Markovits & Guanna Li & Moniek Tromp & Evgeny A. Pidko & Emiel J.M. Hensen & Andreas Jentys & Maricruz Sanchez-Sanchez & Johannes A. Lercher, 2015. "Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol," Nature Communications, Nature, vol. 6(1), pages 1-9, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms8546
    DOI: 10.1038/ncomms8546
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    Cited by:

    1. Hailong Zhang & Peijie Han & Danfeng Wu & Congcong Du & Jiafei Zhao & Kelvin H. L. Zhang & Jingdong Lin & Shaolong Wan & Jianyu Huang & Shuai Wang & Haifeng Xiong & Yong Wang, 2023. "Confined Cu-OH single sites in SSZ-13 zeolite for the direct oxidation of methane to methanol," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Pengfei Xie & Jing Ding & Zihao Yao & Tiancheng Pu & Peng Zhang & Zhennan Huang & Canhui Wang & Junlei Zhang & Noah Zecher-Freeman & Han Zong & Dashui Yuan & Shengwei Deng & Reza Shahbazian-Yassar & C, 2022. "Oxo dicopper anchored on carbon nitride for selective oxidation of methane," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Manav Chauhan & Bharti Rana & Poorvi Gupta & Rahul Kalita & Chhaya Thadhani & Kuntal Manna, 2024. "Tailored pore-confined single-site iron(III) catalyst for selective CH4 oxidation to CH3OH or CH3CO2H using O2," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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